The Raman spectrum of holmquistite, a Li-containing orthorhombic amphibole from Bessemer City, USA has been measured. The OH-stretching region is characterized by bands at 3661, 3646, 3634 and 3614 cm−1 assigned to 3 Mg–OH, 2 Mg + Fe2+–OH, Mg + 2Fe2+–OH and 3 Fe2+–OH, respectively. These Mg and Fe2+ cations are located at the M1 and M3 sites and have a Fe2+/(Fe2+ + Mg) ratio of 0.35. The 960–1110 cm−1 region represents the antisymmetric Si–O–Si and O–Si–O stretching vibrations. For holmquistite, strong bands are observed around 1022 and 1085 cm−1 with a shoulder at 1127 cm−1 and minor bands at 1045 and 1102 cm−1. In the region 650–800 cm−1 bands are observed at 679, 753 and 791 cm−1 with a minor band around 694 cm−1 attributed to the symmetrical Si–O–Si and Si–O vibrations. The region below 625 cm−1 is characterized by 14 vibrations related to the deformation modes of the silicate double chain and vibrations involving Mg, Fe, Al and Li in the various M sites. The 502 cm−1 band is a Li–O deformation mode while the 456, 551 and 565 cm−1 bands are Al–O deformation modes.